Abstract

To better understand the early hydration impact of cement phases on subsequent accelerated carbonation, this study mixed alite (C3S) and belite (β-C2S) with 40 wt% of water for 2, 4, 8, 18 h hydration before exposing to 2 h accelerated carbonation. The results indicated that early hydration exerted a significant impact on C3S (particularly 4–8 h), which accelerated the subsequent carbonation degree (CD) with maximum of 57.27%. Over 8 h, however, packed hydrates impeded CO2 ingress, leading to a decelerated CD and co-existence of different calcium carbonate polymorphs: calcite (dominant for short hydration), aragonite and vaterite (dominant for long hydration). Differently, β-C2S samples with marginal hydrates continuously accelerated CD with time (32.23% after 18 h), and indicated a direct β-C2S carbonation. Detection of calcite and vaterite in carbonated β-C2S samples revealed that carbonates polymorphs varied with calcium silicate and their resulting hydrates participation. This study provides a viable strategy for CO2 storage and microstructure densification, distinct from conventional cement carbonation regime.

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